The development of visible light photoredox catalysis (VLPC) represents intensified efforts to use renewable and low power-consumption light sources to drive the reactions that produce fuels and fine chemicals. Colloidal semiconductor nanocrystals (NCs) are advantageous when compared to molecular VLPC photocatalysts, because they have synthetically tunable size-dependent absorption spectra, surfaces that are amenable to chemical functionalization, and enhanced photostability. Molecular photocatalysts also cannot stabilize freely diffusing redox intermediates in solution, so they are limited to initiating single-electron transfer reactions. NCs are capable of facilitating multi-electron reactions by stabilizing the redox intermediates that adsorb to their surfaces. Photoexcited electrons and holes must separate across the nanocrystal surface during photocatalysis, precluded often by charge recombination, especially in metal oxides. Transition metal complexes covalently bonded to the NC surfaces may enhance the rate of charge separation and increase the lifetime of the charge-separated state. Cooperative binding geometries involving the transition metal complex, the NC surface atoms and reactant molecules may also be possible. Strategies for covalent attachment of polypyridyl Ru(II) and Co(III) complexes to metal oxide (In2O3, Sn:In2O3, Fe2O3) NCs using compact bridging ligands will be presented. The influence that the transition metal complexes have on the NCs photophysical properties and colloidal stability will be highlighted.

Nanocrystal-molecule hybrid materials for photoredox catalysis

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.